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Among the 'beyond Li-ion' battery chemistries, nonaqueous Li-O$_2$ batterieshave the highest theoretical specific energy and as a result have attractedsignificant research attention over the past decade. A critical scientificchallenge facing nonaqueous Li-O$_2$ batteries is the electronically insulatingnature of the primary discharge product, lithium peroxide, which passivates thebattery cathode as it is formed, leading to low ultimate cell capacities.Recently, strategies to enhance solubility to circumvent this issue have beenreported, but rely upon electrolyte formulations that further decrease theoverall electrochemical stability of the system, thereby deleteriouslyaffecting battery rechargeability. In this study, we report that a significantenhancement (greater than four-fold) in Li-O$_2$ cell capacity is possible byappropriately selecting the salt anion in the electrolyte solution. Using$^7$Li nuclear magnetic resonance and modeling, we confirm that thisimprovement is a result of enhanced Li$^+$ stability in solution, which in turninduces solubility of the intermediate to Li$_2$O$_2$ formation. Using thisstrategy, the challenging task of identifying an electrolyte solvent thatpossesses the anti-correlated properties of high intermediate solubility andsolvent stability is alleviated, potentially providing a pathway to develop anelectrolyte that affords both high capacity and rechargeability. We believe themodel and strategy presented here will be generally useful to enhance Coulombicefficiency in many electrochemical systems (e.g. Li-S batteries) whereimproving intermediate stability in solution could induce desired mechanisms ofproduct formation.

Enhancing electrochemical intermediate solvation through electrolyte anion selection to increase nonaqueous Li-O$_2$ battery capacity